Method of manufacturing graphite.



liurrnn g'rn'rits EDNARD GOODRICH ACHESON, OF BUFFALO, NEW

METHQD OF MANUFACTUWNG GRAPHWEQ SPECIFICATION forming part of Letters Patent No. 645,285, dated March 13, 1900.

"Application fine simmer 30, 1899,

To (all whom, ('0' may mnccrn:

Be it known that I, EDWARD GooDRIciI ACH'ESON, a citizen of the United States, re-

siding at Buffalo, in the county of Erie and State 0'' New York, have invented certain new and useful Improvements in the Methods of Manufacturing Graphite, of which the follow ing is a specification.

In my prior patent, No. 568,323, in which I claim, broadly, themanufacture of graphite by decomposition of a carbid, and to which my present invention is subordinate,l describe particularly the treatment of carbonaceous materials containing sufficient impurities that will makcchcmical eompoundetherewith to initially form true fixed carbide of all the contained carbon not utilized in the reduction of the oxide of the impurities, and where the amount of impurities in the original carbonaceous material is notsuiiicient to fix all of the carbon in a true carbid additional impurities are added thereto, and where a carbonaceous material contains an excess of these impurities a material rich in carbon is added in order that the proper proportions may be established, the object beiug to operate upon a mixture of approximately theoretical chemical composition for the initial formation of carbide of the carbon and the associated impurities, and the process further provides that the carbon in the carbids' thus formed is disassociated or separated therefrom into the graphitic form,while the other elements of the carbid are volatilized. Thus it will be seen that the process primarily provides for the formation of carbids of all, or approximately all, of the material operated upon not disposed of in the reduction of the metallic oxids prior to the liberation of the carbon in the graphitic state, and this necessitates the presence of practically the theoretical proportion of silicon or other element forming the carbid, as illus tratcd in the patcntspcciiication, taking, for example, fifty parts, by weight, of coke'and lifty parts, by weight, of silica, the excess in carbon being intended to combine with the oxygen of the silica, the theoretical proportions beingapproximately thirty partsof carbon and seventy of silicon.

In my Patent No. 617,979 I have described and claimed the method of manufacturing rial No. 732,202. (lie specimens.)

articles containinga desired amount of graphite, in which I made use of amorphous CB1:- bon mixed. with some material capable of combining with the carbon and-to which is added a proper binding material, and the article was then molded from the mixture and subjected to a temperature sufiicicntiy high and-for sufiicient length of time and under such conditions as to-ceuse more or less of the carbon in the article to be c'ouvertedinto graphite.

In carrying out this process I described the use of amorphous carbon, and to this carbon ll added impurities capable of chemically combining therewith in such amount as found necessary for the production of the desired amount of graphite, and the process further provides for the chemical association of the impurities with successive portions of the carbon in a progressive manner and the conversion of more or less of the carbon-into graphite, the amount of graphite produced in the article'by the process depending upon the character of the original amorphous carbon and the characterand amount of impurities added therewith. I have discovered thatthe amount of graphite produced in such articles by progressive formation and decomposition of the carbide further depends upon the degree of perfection of the intermingling of the carbon and the associated impurities,

"so that even under the best attainable artificisl mixing or distributing the action would be more or less irregular and incomplete. I have further discovered that a higher degree of perfection in making graphite by the progressive action-above described can be obtained by employing certain carbonaceous materials wherein the impurities are naturally and inherently distributed and which afford the necessary conditions for the formation of graphite from the contained carbon, in that the character, quantity,andi1atural and inherent distribution of the associated impurities are such as to produce better results than I have been able to obtain by artificial mixturcsyund, moreover, I have discovered that a comparativcly-siunll percentagcof such naturally-distrihuted and inhercut impurities will produce a practically-coinplote conversion of the carbon not lost in the volatile chemical products, owing to the accu- 7 tion ofimpurities capable of forming rate or even natural distribution of the impurities throughout the body of carbonaceous mo.- ierial. Thus Ihsve found that an anthracite coei which contains 5. 783 per cent. oi ash, consisting largely of silica, alumina, and iron oxids, is converted into a practically-pure graphits by treatment under my process hereinbe fore described and that the contained ash is found by analysis to have been reduced to 0.033 per cent. I l have also discovered that use can he made of carbonaceous nihterial in general which (like anthracite coal) contains in the respective pieces or particles thereof, of whatever size or fineness of subdivision, less carbid-forming impurities than will convert the whole of said pieces or particles respectively into fixed carbid. Thus use can be made, forinstancc, of lignite, pent,otlier nonceking coals, some forms of wood or the charconls produced therefrom and contuiningm sufficient percentage of ash, such as willow, and all those carbon accous materials containing a substantially-uniform naturel (lisi "l and that may he charred in the nutu withoutdestroying the relative posil the carbon and associated impurities tiuguished,-for example, from a on tuminoii's coal. in which the metallic oxids tend to settle into the lower layers, precincing ain uneven distribution when such coal is sub'ecied to heat.

ypresent invention is based upon said discoveries and relates to a process of prodncing graphite, its object being to produce graphite cheaply and in a practically-pure state; and it consists, briefly stated, in the method of procedure substantially as hereinafter more particularly setforth and claimed, whereby pieces or particles of certain cairbo naceous materials-such as anthracite coal, other non-ceking coal, willow-charcoal, nhd others, as specified-arc converted into graphite in a practically-uniform condition throughout.

-As illustrative of the carrying out of my present invention, I take anthracite coal of any desired size, or by preference I takethe refuse'coal, which is known as anthracite culm, and subject it to a sufiiciently-high temperature for a suificient length of timeto effect the volntilization of the impurities. A reaction occurs, however, prior to the vola- Y tilization of the impurities between them and.

the associated carbon, the formation and destruction of a carhid or carbide-such, for in-.

stance, as carhid of silicon or oer-bid of iron; but, as heretofore explained, the amount of impurities not being sufficient to form a carbid of all the carbon "at one and the. same time a catalytic or progressive action occurs.

Owing to the fact; that in these carbonaceous materials the distribution of the impurities is natural'nnd practically uniform, o catelyt-ic action is facilitated and practically all of the carbon. can be converted into the graphitic form before the final volatilization and verted;

semen escape of ihe impurities, and this even al.

though a relatively-smellamount of impurities is present.

in practically carrying out this process I have made use oi" on electric furnace which the materials are protected from atmospheric influences and in which the materials cam be heated to and maintained at a high tempera- In body of the carbonaceous material to be trcaied being placed in such furnace around -a central condu'etingcorc, which, however,

may with advantage be oi less diameter than is preferably used in the cnrooruniluin-furmice. The ends of thecorc are connected with the usual electrodes and the current is passed through the same, raising the contents oi". Lhc'iurnece to an intense heat and accomplishing the desired reactions in that portion of ihe charge lying near the core. The temperature which is attained is above the vaporiziugpointol' the contained impurities, for Analysis shows that the ash content of the graphite is less than than oi the anthracite or like material treated. Moreover, spectroscopic examination of vapors csca-pingduring the operntion$how the presence of metals therein. In thus proceeding the heat which effects the conversion 'into graphite of the non-coking coal or other specified materiel, whether said heat be produced primarily in the conducting-core or primarily in the inn.- tcrinl to he converied, is generated electrically within the mass ol'snid material, so that the vapors produced are those of substances forming part of the uon-caking coal or other ing lay-the aid of the impurity naturally pres ent insaid coal or other specified material irrespective of the generation of the electrical heat withiu the mass of material to be con- Moreorer, it is 'a further advantage and special improvement to supply the electricalheat by the aid of a conductor of less resistance than the non-coking coal"or other specified material and in contact therewith and formed best (although notnccessarily'to thecxclusion of other materials) oligraphitc in a solid or loose condition. A con'ductorof this description is employed in the before mentioned curhorundum-furnace. (See my Patent No. 492,767, dated February 28, 1893.) One advantage of this mode of electric heating is the facility 'ivhich it affords for controlling the temperature. It also permits the heating action to be extended over a longer distance than would be practicable without its aid.

So far as I am aware ell non-coking coal contains inherent impurities capable of forming carbids, but less in amount than enough to convert the whole piece into said carbids and naturally distributed with substantial uniformity in the piece; but whether so or not it must be understood that the non-caking coal of the hereinafter-written claims is intended to be of this description. It will be understood that the expression non-caking coal wherever it occurs in any of said claims is intended to include other like carbonaceous materials, as hereinbefore set forth.

What I claim is- 1. The method herein described of making graphite, consisting in treating an aggregation of pieces or particles of carbonaceous material of which the said pieces or particles respectively contain inherent impurities capable of forming carbids but less in amount than enough to convert the whole of the respective pieces or particles into said carbids and naturally distributed with substantial uniformity in the piece and which can be heated to a eharring temperature without destroying the relative positions of the carbon and such associated impurities, by heating said material to a high temperature and continuing such heating until the individual pieces have been progressively converted into graphite in greater proportion than would be produced by decomposition of the relativelysmall amount of fixed carbid capable of being formed by the impurities naturally present in said pieces, substantially as described.

2. The method herein described of making graphite which consists in heating to a high temperature while protected from atmospheric influence, an aggregation of pieces or particles of non-caking coal, of which the said pieces or particles contain inherent impuritiescapable of forming carbids but less in amount than enough to convert the whole of the respective pieces or particles into said carbids and naturally distributed with substantial uniformity in the piece and which can be heated to a charrin g temperature without destroying the relative positions of the carbon and such associated impurities, without previously changing the natural ash content thereof and thereby converting the pieces into graphite, substantially as described.

3. The method herein described of making graphite, which consists in heating non-caking coal, the pieces or particles of which contain inherent impurities capable of forming carbids, but less in amount than enough to convert the whole of the respective pieces or particles into said carbids and naturally distributed with substantial uniformity in the piece and which can be heated to a charring temperature without destroying the relative positions of the carbon and such associated impurities, to a high temperature by passing electricity through said coal and thereby generating electrically within the same the heat necessary for making the graphite, substantially as described.

4:. The method herein described of making graphite, which consists in heating non-caking coal, the pieces or particles of which contain inherent impurities capable of forming carbids but less in amount than enough to convert the whole of the respective pieces or particles into said carbids and naturally distributed with substantial uniformity in the piece and which can be heated to a charring temperature without destroying the relative positions of the carbon and such associated impurities, to a high temperature by passing electricity through a conductor of less resistance than said coal, and in contact therewith, and thereby generating electrically by the aid of said conductor the heat necessary for making the graphite, substantially as described.

In testimony whereof I have signed my name to this specification in the presence of two subscribing witnesses.

EDWARD GOODRICH ilCHESON.

Witnesses:

THOMAS W. BAKEWELL, FRANK L. FREEMAN. 

